WO1985000377A1 - Composition et procede de capture du soufre - Google Patents

Composition et procede de capture du soufre Download PDF

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Publication number
WO1985000377A1
WO1985000377A1 PCT/SE1984/000259 SE8400259W WO8500377A1 WO 1985000377 A1 WO1985000377 A1 WO 1985000377A1 SE 8400259 W SE8400259 W SE 8400259W WO 8500377 A1 WO8500377 A1 WO 8500377A1
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WO
WIPO (PCT)
Prior art keywords
sulphur
weight
fuel
composition
capturing
Prior art date
Application number
PCT/SE1984/000259
Other languages
English (en)
Inventor
Mait Mihkel Mathiesen
Olle NYSTRÖM
Original Assignee
Ab Carbogel
Berol Kemi Aktiebolag
Priority date (The priority date is an assumption and is not a legal conclusion. Google has not performed a legal analysis and makes no representation as to the accuracy of the date listed.)
Filing date
Publication date
Family has litigation
First worldwide family litigation filed litigation Critical https://patents.darts-ip.com/?family=10545698&utm_source=google_patent&utm_medium=platform_link&utm_campaign=public_patent_search&patent=WO1985000377(A1) "Global patent litigation dataset” by Darts-ip is licensed under a Creative Commons Attribution 4.0 International License.
Application filed by Ab Carbogel, Berol Kemi Aktiebolag filed Critical Ab Carbogel
Priority to DE8484902837T priority Critical patent/DE3468902D1/de
Priority to AT84902837T priority patent/ATE32096T1/de
Publication of WO1985000377A1 publication Critical patent/WO1985000377A1/fr
Priority to DK85185A priority patent/DK85185D0/da

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Classifications

    • C—CHEMISTRY; METALLURGY
    • C10—PETROLEUM, GAS OR COKE INDUSTRIES; TECHNICAL GASES CONTAINING CARBON MONOXIDE; FUELS; LUBRICANTS; PEAT
    • C10L—FUELS NOT OTHERWISE PROVIDED FOR; NATURAL GAS; SYNTHETIC NATURAL GAS OBTAINED BY PROCESSES NOT COVERED BY SUBCLASSES C10G, C10K; LIQUEFIED PETROLEUM GAS; ADDING MATERIALS TO FUELS OR FIRES TO REDUCE SMOKE OR UNDESIRABLE DEPOSITS OR TO FACILITATE SOOT REMOVAL; FIRELIGHTERS
    • C10L1/00—Liquid carbonaceous fuels
    • C10L1/32—Liquid carbonaceous fuels consisting of coal-oil suspensions or aqueous emulsions or oil emulsions
    • C10L1/326—Coal-water suspensions

Definitions

  • DE 2,947,788 which describes a semiliquid fuel con ⁇ taining coal, water and certain thickening salts, such as sodium, potassium or calcium nitrates.
  • the mixture may also include emulsified oil, anionic soap being added as emulsifier.
  • GB 2,009,783 which relates to a composition of a solid combustible material, such as coal, and a liquid fuel, such as gasoline, oil etc., and a gelling and ash modifiying agent which is selected for example among metallo-organic compounds or inorganic compounds, such as pyrogenic silica, calcium oxide, calcium hydroxide, calcium carbonate etc.
  • the modifying agent shall only keep the fuel particles apart and modify the melting point of the slag formed and has no sulphur-capturing function.
  • the fuel composition further is devoid of dispersants.
  • GB 2,009,782 which substantially corresponds to the above-mentioned GB 2,009,783, with the difference, however, that one has added a special gelling agent
  • OMPI which is combustible and for instance consists of car ⁇ bon black, synthetic gums and resins.
  • US 3,948,617 which describes the treatment of gaseous, liquid or solid fuels, such as coal powder, with sulphur neutralising alkali to neutralise sulphur dioxide which is formed during the combustion of the fuel.
  • the alkali can be oxides of sodium, potassium, lithium, calcium, magnesium or aluminium, preference being given to sodium, potassium and'lithium oxide.
  • SE 75 11947-9 which describes a fuel of coal particles in a water-in-oil emulsion, to which finely divided alkali, such as lime, can be added to eliminate sulphur dioxide at the combustion of sulphurous fuel.
  • US 4,396,397 which describes a fuel which to the major part consists of fuel oil and to a smaller part of coal powder and an addition of 0.1-5% by weight of calcium acetate to reduce S0 2 .
  • EP 00 66817 which describes a fuel which consists of coal powder, oil and water and a dispersion stabi ⁇ lising agent.
  • the stabilising agent may int.al. be graphite or a water insoluble, inorganic hydroxide, such as silica, aluminium hydroxide, ferric hydroxide or titanium hydroxide.
  • the present invention relates to the capture of sulphur emanating from burning particulates prior to formation of gaseous sulphur oxides which become diluted in the gaseous phase during and after combus ⁇ tion. This can be achieved by depositing a sulphur captor on or sufficiently near the burning carbonaceous fuel particles, thereby utilizing the local chemical potential in the formation of (locally) stable sulphides
  • OMPI . _ at relatively low oxygen potentials.
  • sulphur is captured as solid sulphide.
  • the temperature drops as the solid combustion residue leaves the flame and the local oxygen potential rises (as a result of carbon burn-out) sul ⁇ phate formation occurs.
  • Some of the sulphide formed also reacts with oxygen to form sulphate.
  • the- present invention relates to a method of capturing sulphur emanating from burning carbonaceous fuel particles prior to the point at which gaseous sulphur oxides are formed wherein
  • an aqueous fuel composition which comprises about 60-80% by weight of carbonaceous fuel particles with an ash content of below about 5% by weight, on a dry basis, about 0.05-2.0% by weight of a flow-enhancing chemical which includes a non-ionic dispersant, and a liquid carrier phase consisting es ⁇ sentially of water, and
  • a sulphur-capturing substance which includes a compound, of a metal with a higher affinity to sulphur ' than Fe is added to said composition in an amount of about 0.1-5% by weight of the compound calculated as pure metal upon total solid fuel weight.
  • the invention also relates to an aqueous fuel composition in which sulphur emanating from burning carbonaceous fuel particles is captured prior to the point at which gaseous sulphur oxides are formed, where ⁇ in the composition comprises
  • a sulphur-capturing substance which includes a compound of a metal with a higher affinity to sulphur than Fe in an amount of about 0.1-5% by weight of the compound calculated as pure metal upon total solid fuel weight.
  • the par- ticulate carbonaceous fuel has an ash content of below about 5% by weight, on a dry basis. This is important in order to avoid slag formation problems due to the sulphur captor added.
  • the requirement for a low ash content implies that the carbonaceous fuel, unless it consists of pure coal only, has to be purified before it can be used for the purposes of the invention.
  • Suitable captors are compounds of sulphide-forming metals such as calcium, magnesium, manganese, etc. It is essential that the captor be added to the fuel in such a way that the captor is well dispersed in the
  • the amounts in which the captor is added to the fuel are limited minimally by the amount of sulphur that is- desired to be eliminated from the off gas.
  • About 0.1 weight percent, preferably 0.3 weight percent, of the captor as pure metal based upon total solid fuel weight is a practical lower limit.
  • the upper limit is indicated by the amount at which the captor begins to impede the combustion reaction, usually at or below about 5 weight percent, the preferred lower limit being about 0.5 percent.
  • captor should be added in such a way to the fuel that sufficient proxi ⁇ mity between captor and fuel particle can be achieved.
  • This can ideally be achieved by adding the captor com- pound to a mixture of particulate coal and a liquid (essentially water) in which the coal is dispersed prior to passing the mixture through a burner device which atomizes the mixture, creating a spray of droplets con- taining one or more coal particles, captor and liquid.
  • mixtures suitable for effi ⁇ cient energy conversion with simultaneous sulphur cap ⁇ ture can effectively comprise-: a) Solid particulate carbonaceous fuel containing sulphur, such as coal of any rank, coke, solid refinery by-products or other sulphur bearing carbonaceous solids, and b) Liquid carrier phase consisting essentially of water, and c) Soluble and/or fine particulate compounds of a sulphur capturing, sulphide-forming substance which includes a compound of a metal with a higher affinity to sulphur than Fe.
  • sulphur capturing substances are Ca(0H)_, CaCO ⁇ , Mg(OH) , MnO, or any others which can be selected by those skilled in the art.
  • the sulphur captor added does not consist of substances forming low melting slag products which give rise to problems at the combustion. These undesired substances above all consist of compounds of the alkali metals sodium, potassium and lithium which are not there ⁇ fore comprised by the present invention. It is further required for the purposes of the invention that the sulphur captor added shall not in itself have an environment contaminating effect or at
  • MPI a combustion of the fuel give rise to environment con ⁇ taminating products.
  • the anions be of such nature that the burning of the fuel containing the captor compound does not contribute to environmental pollution or combustion equipment corro- sion or fouling.
  • An example of a harmful anion is sul ⁇ phate.
  • certain metal ions can be harmful in that they may cause e.g. boiler corrosion or fouling.
  • Such metals are e.g. sodium and potassium, as is well known to those skilled in the art.
  • the sulphur captor according to the invention preferably consists of metal oxides, metal hydroxides or metal carbonates, while such metal compounds as nitrates, sulphates, chlorides fall outside the scope of the in ⁇ vention.
  • the sulphur capturing substance is selected from the group c'onsisting of hydroxides, oxides and carbonates of calcium, magnesium and manga ⁇ nese. It is required that the various components should be blended together so as to achieve efficient disper ⁇ sion.
  • coal or other carbo ⁇ naceous solid fuel particles of maximum size 20 to 500 microns are admixed with water, flow-enhancing che- ical additives such as surface active water-soluble compound, and sulphur captor such as Ca(OH) of essen ⁇ tially smaller particle size than 10 microns.
  • the pH of the water can be varied so as to provide for suit ⁇ able solubility of the captor, e.g. CaOH, therein.
  • the sulphur captor when in solid form has a particle size of below 10 urn. Furthermore, it is advantageous if the sulphur captor is soluble, wholly or partly, in the carrier liquid used (water or essentially water) .
  • the aqueous carrier liquid is evaporated and the carbonaceous fuel particles are surrounded by a coat of aqueous carrier liquid which continuously shrinks because of evaporation.
  • the sulphur captor dis ⁇ persed or dissolved in the carrier liquid will as a result deposit on the surface of the fuel particles and be in intimate contact with them when the carrier liquid has been wholly, evaporated and the combustion of the particles begins.
  • the local oxygen potential at the particle surface is low and the for ⁇ mation of solid sulphide is favoured at the reaction with the sulphur captor.
  • the carrier liquid is a com ⁇ bustible liquid, such as oil
  • the above-mentioned eva ⁇ poration process with the deposition of the sulphur captor in intimate contact with the fuel particles will not come about, but the carrier liquid is burnt also itself simultaneously with the fuel particles.
  • the solid fuel particles contain minimum amounts of non-combustible impurities which may combine with the sulphur captor during and after combustion, thereby creating low-melting compounds which might adversely affect the heat-transfer process.
  • coal it is essential that the coal be physically beneficiated prior to combustion in order to minimize captor/coal ash reactions at high temperature. Such physical beneficiation normally lowers the acidity of the ash composition and therefore limits the possibility of low-melting captor/coal ash combus ⁇ tion residue " formation.
  • the sulphur captor may be combined into the slurry at any point prior to combustion because the sulphur- capturing process occurs during and, to a minor extent, after combustion of the fuel, whereafter the captured sulphur is removed in the removal of particulates from the off gas stream.
  • Usual relative amounts of the fuel mixture compo ⁇ nents are: a) -Carbonaceous fuel 60-80%, preferably 70 to 80%, by weight. b) Aqueous liquid, preferably water, 20-40% by weight, preferably 20 to 30% by weight. c) Sulphur captor, preferably a calcium compound, most preferably Ca(OH)_, 0.1 to 5% by weight of the capturing compound, calculated as pure metal based upon total solid fuel weight, in whatever form it may be added. d) Flow-enhancing chemical, 0.05 to 2.0 percent by weight. The flow-enhancing chemical must be of such a na ⁇ ture that the sulphur captor compound does not nega ⁇ tively interact with it, i.e.
  • the flow-enhancing chemical must consist of or at least include as a major constituent a non-ionic dispersant.
  • Preferred types of flow-enhancing chemicals are water soluble nonionic surface active compounds such as ethyloxylated nonylphenol or dinonyl- phenol with 40 to 90 repeated ethylene oxide units, especially when using sulphur captors such as Ca(OH) and CaCO... The selection of other such suitable chemicals and sulphur captors will be readily apparent to those skilled in the art.
  • a solid captor such as dolomite powder, or other compound containing the
  • OMPI sulphide and sulphate forming metal(s) in the form of dispersed captor slurry, com ⁇ prising, for instance, sulphur captor, dispersant and water.
  • Dispersing the sulphur captor in the liquid phase of a solid fuel/liquid slurry be it in the form of a fine particulate (CaCO. , CaCO-* MgCO , Ca(OH) , etc.) or in the form which is soluble in one or . more liquids of the said"liquid phase.
  • a fine particulate CaCO. , CaCO-* MgCO , Ca(OH) , etc.
  • the sulphur captor will be well and evenly distri ⁇ minded in the whole volume wherein combustion occurs and sulphur is released.
  • the fraction of the captor deposited on the fuel particles is particularly efficient in capture of the sulphur as sulphide at the high combustion temperature and low oxygen potential on or near the solid fuel particle.
  • MeO can be Ca, Mg, Mn, or any other sulphide- forming metal with higher affinity to sulphur than Fe, but Ca is preferred. -However, as mentioned before, the metal shall not form low-melting slags during the combustion, and therefore alkali metals and their compounds are not comprised by the inven ⁇ tion.
  • a major fraction of the sulphur originally present in the fuel is chemical ⁇ ly bound to the particulate material and only a minor fraction is present in the gaseous phase as SOx.
  • the particulates are removed from the off gas stream using, for example, baghouses or electro- static precipitators, whereby only minimal amounts of sulphur are released to the atmosphere.
  • the solid fuel originally has an ash content of more than 5% by weight it must first be subjected to physical and, where appli ⁇ cable, chemical cleaning prior to its incorporation into the slurry which is to be atomized and burnt with added sulphur captor.
  • This reduces impurities in the solid fuel such as, i the case of coal, inorganic sul ⁇ phur and other inorganic species thereby a) reducing the requirement for sulphur captor and b) reducing the disadvantages of handling an impure fuel and combustion residue from impure fuel.
  • This cleaning also means, that the sulphur captor may increase the temperature at which the ash melts in the furnace, thereby reducing the slagging tendency of the fuel.
  • fuels with higher ash contents may give less desirable results, e.g. CaO, or other MeO, may combine with fuel ash to form low melting oxide mixtures (e.g. basic CaO com ⁇ bining with acidic SiO-) resulting in slagging problems impeding heat transfer processes in the combustion ap ⁇ paratus and inhibition of sulphur capture, it being commonly recognized that extensive coal cleaning to very low ash levels removes the acidic ash-forming com ⁇ ponents to a greater extent than the basic components..
  • low melting oxide mixtures e.g. basic CaO com ⁇ bining with acidic SiO-
  • EXAMPLE 1 200 kg of a coal/water slurry containing 72 weight percent coal was admixed with 3 kg of calcium hydroxide powder (less than 10 u size). The coal contained in the slurry was of Canadian origin (Cape Breton Develop ⁇ ment Corporation, Harbour seam coal) and was subjected to physical cleaning prior to incorporation in the aqueous slurry. The coal particle size was less than 200 urn and the approximate analysis was as follows:
  • the slurry was fired in a vertically fired oil- design fire-tube boiler at 1.4 M (thermal) load (ap- proximately 60% of full load when oil fired) .
  • the off gas analysis showed that only approximately 21.9% of the sulphur originally present in the fuel occurred in the gaseous phase as SO-/SO.., indicating that an 82% efficiency in sulphur capture was achieved.
  • the use of calcium hydroxide in the slurry fuel has accordingly been shown to be a very cost effective method of limiting sulphur oxide emission to the atmos- phere when firing this particular type of coal/water slurry.
  • the low coal ash content contributed to the absence of any boiler slagging problems during the test. -
  • Example 1 is repeated with the difference that mag ⁇ nesium hydroxide is substituted for the calcium hydroxide. The results obtained are essentially the same.
  • EXAMPLES 3 and 4 are repeated with the difference that mag ⁇ nesium hydroxide is substituted for the calcium hydroxide. The results obtained are essentially the same.
  • Example 1 is repeated with the difference that formic acid is added to the slurry to effect increased dissolution of the calcium hydroxide powder. This will also somewhat reduce the viscosity of the slurry. The sulphur capturing results are essentially the same.

Abstract

Composition et procédé de capture du soufre émanant de particules d'un combustible carbonné en combustion d'une composition de combustible aqueuse comprenant environ 60-80% en poids de particules de combustible carbonné avec une teneur en cendres inférieure à 5% environ en poids calculée à l'état sec, environ 0,05-2,0% en poids d'un agent chimique améliorant l'écoulement qui comprend un agent de dispersion non ionique, et une phase porteuse liquide consistant essentiellement en eau. Le soufre est capturé avant la formation d'oxydes de soufre gazeux qui se diluent sur la phase gazeuse pendant et après la combustion, et consiste à introduire un capteur de soufre choisi de préférence parmi des hydroxydes, des oxydes ou des carbonates de calcium ou de magnésium à une proximité des particules de combustible carbonné en combustion facilitant la réaction, utilisant ainsi un potentiel chimique local dans la formation de sulfure localement ou relativement stable à des potentiels d'oxygène relativement faibles, le soufre étant capturé pendant la phase de combustion sous forme de sulfure solide et par conséquent, lorsque la température chute lorsque le résidu solide de combustion quitte la flamme et que le potentiel d'oxygène local augmente, et que se produit une formation de sulfate, sous la forme de sulfate. La quantité de soufre dans le gaz libéré de la combustion est par conséquent considérablement réduite selon le procédé de la présente invention.
PCT/SE1984/000259 1983-07-14 1984-07-11 Composition et procede de capture du soufre WO1985000377A1 (fr)

Priority Applications (3)

Application Number Priority Date Filing Date Title
DE8484902837T DE3468902D1 (en) 1983-07-14 1984-07-11 A composition and a method of capturing sulphur
AT84902837T ATE32096T1 (de) 1983-07-14 1984-07-11 Zusammensetzung und verfahren zum auffangen von schwefel.
DK85185A DK85185D0 (da) 1983-07-14 1985-02-25 Middel og fremgangsmaade til indfangning af svovl

Applications Claiming Priority (2)

Application Number Priority Date Filing Date Title
GB838319033A GB8319033D0 (en) 1983-07-14 1983-07-14 Sulphur capture
GB8319033 1983-07-14

Publications (1)

Publication Number Publication Date
WO1985000377A1 true WO1985000377A1 (fr) 1985-01-31

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Application Number Title Priority Date Filing Date
PCT/SE1984/000259 WO1985000377A1 (fr) 1983-07-14 1984-07-11 Composition et procede de capture du soufre

Country Status (9)

Country Link
US (1) US4783197A (fr)
EP (1) EP0149664B1 (fr)
JP (1) JPS60502157A (fr)
CA (1) CA1245449A (fr)
DE (1) DE3468902D1 (fr)
DK (1) DK85185D0 (fr)
GB (1) GB8319033D0 (fr)
IT (1) IT1175566B (fr)
WO (1) WO1985000377A1 (fr)

Cited By (2)

* Cited by examiner, † Cited by third party
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EP0158587A2 (fr) * 1984-04-10 1985-10-16 MANNESMANN Aktiengesellschaft Procédé d'abaissement l'émission de polluants dans des unités de combustion
DE3804834A1 (de) * 1987-02-17 1988-08-25 Intevep Sa Verfahren zum herstellen bzw. verbrennen eines brennstoffes sowie kohlenwasserstoff-brennstoff dafuer

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IT1233848B (it) * 1988-01-21 1992-04-21 Snam Progetti Procedimento per la preparazione di una sospensione acquosa di carbone o di petcoke ad alta concentrazione
UA78508C2 (en) * 2001-03-28 2007-04-10 Sgt Technology Holdings Llc Method for the treatment of coal with a high content of sulphur, method for producing energy, coal with high content of sulphur and unit for the coal treatment with high content of sulphur
US20060064927A1 (en) * 2004-09-27 2006-03-30 Farone William A Process for treating coal with a magnetic gradient to reduce sulfur dioxide emissions
US20100263577A1 (en) * 2009-04-21 2010-10-21 Industrial Accessories Company Pollution abatement process for fossil fuel-fired boilers
FI123354B (fi) * 2010-12-20 2013-03-15 Foster Wheeler Energia Oy Järjestely ja menetelmä kiinteän polttoaineen kaasuttamiseksi
MX2018015979A (es) 2016-06-29 2019-05-30 Cemex Res Group Ag Metodo para reducir acumulaciones, incrustaciones y formacion de anillos en la produccion de clinker.

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Cited By (3)

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Publication number Priority date Publication date Assignee Title
EP0158587A2 (fr) * 1984-04-10 1985-10-16 MANNESMANN Aktiengesellschaft Procédé d'abaissement l'émission de polluants dans des unités de combustion
EP0158587A3 (en) * 1984-04-10 1986-02-05 Mannesmann Aktiengesellschaft Process for lowering the emission of pollutants in combustion units
DE3804834A1 (de) * 1987-02-17 1988-08-25 Intevep Sa Verfahren zum herstellen bzw. verbrennen eines brennstoffes sowie kohlenwasserstoff-brennstoff dafuer

Also Published As

Publication number Publication date
DE3468902D1 (en) 1988-02-25
CA1245449A (fr) 1988-11-29
DK85185A (da) 1985-02-25
IT8421876A0 (it) 1984-07-12
DK85185D0 (da) 1985-02-25
US4783197A (en) 1988-11-08
EP0149664B1 (fr) 1988-01-20
IT1175566B (it) 1987-07-01
EP0149664A1 (fr) 1985-07-31
JPH0377237B2 (fr) 1991-12-09
IT8421876A1 (it) 1986-01-12
GB8319033D0 (en) 1983-08-17
JPS60502157A (ja) 1985-12-12

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